Zero-Point Spin-Fluctuations of Single Adatoms.

Stabilizing the magnetic signal of single adatoms is a crucial step toward their successful usage in widespread technological applications such as high-density magnetic data storage devices. The quantum mechanical nature of these tiny objects, however, introduces intrinsic zero-point spin-fluctuations that tend to destabilize the local magnetic moment of interest by dwindling the magnetic anisotropy potential barrier even at absolute zero temperature. Here, we elucidate the origins and quantify the effect of the fundamental ingredients determining the magnitude of the fluctuations, namely, the (i) local magnetic moment, (ii) spin-orbit coupling, and (iii) electron-hole Stoner excitations. Based on a systematic first-principles study of 3d and 4d adatoms, we demonstrate that the transverse contribution of the fluctuations is comparable in size to the magnetic moment itself, leading to a remarkable ≳50% reduction of the magnetic anisotropy energy. Our analysis gives rise to a comprehensible diagram relating the fluctuation magnitude to characteristic features of adatoms, providing practical guidelines for designing magnetically stable nanomagnets with minimal quantum fluctuations.

Kagomerization of transition metal monolayers induced by two-dimensional hexagonal boron nitride.

The kagome lattice is an exciting solid state physics platform for the emergence of nontrivial quantum states driven by electronic correlations: topological effects, unconventional superconductivity, charge and spin density waves, and unusual magnetic states such as quantum spin liquids. While kagome lattices have been realized in complex multi-atomic bulk compounds, here we demonstrate from first-principles a process that we dub kagomerization, in which we fabricate a two-dimensional kagome lattice in monolayers of transition metals utilizing an hexagonal boron nitride (h-BN) overlayer. Surprisingly, h-BN induces a large rearrangement of the transition metal atoms supported on a fcc(111) heavy-metal surface. This reconstruction is found to be rather generic for this type of heterostructures and has a profound impact on the underlying magnetic properties, ultimately stabilizing various topological magnetic solitons such as skyrmions and bimerons. Our findings call for a reconsideration of h-BN as merely a passive capping layer, showing its potential for not only reconstructing the atomic structure of the underlying material, e.g. through the kagomerization of magnetic films, but also enabling electronic and magnetic phases that are highly sought for the next generation of device technologies.

Generalization of the Landau-Lifshitz-Gilbert equation by multi-body contributions to Gilbert damping for non-collinear magnets.

We propose a systematic and sequential expansion of the Landau-Lifshitz-Gilbert equation utilizing the dependence of the Gilbert damping tensor on the angle between magnetic moments, which arises from multi-body scattering processes. The tensor consists of a damping-like term and a correction to the gyromagnetic ratio. Based on electronic structure theory, both terms are shown to depend on e.g. the scalar, anisotropic, vector-chiral and scalar-chiral products of magnetic moments:ei⋅ej, (nij⋅ei)(nij⋅ej),nij⋅ (ei×ej),(ei⋅ej)2,ei⋅ (ej×ek) …, where some terms are subjected to the spin-orbit fieldnijin first and second order. We explore the magnitude of the different contributions using both the Alexander-Anderson model and time-dependent density functional theory in magnetic adatoms and dimers deposited on Au(111) surface.

Interplay of magnetic states and hyperfine fields of iron dimers on MgO(001).

Individual nuclear spin states can have very long lifetimes and could be useful as qubits. Progress in this direction was achieved on MgO/Ag(001) via detection of the hyperfine interaction (HFI) of Fe, Ti and Cu adatoms using scanning tunneling microscopy. Previously, we systematically quantified from first-principles the HFI for the whole series of 3d transition adatoms (Sc-Cu) deposited on various ultra-thin insulators, establishing the trends of the computed HFI with respect to the filling of the magnetic s- and d-orbitals of the adatoms and on the bonding with the substrate. Here we explore the case of dimers by investigating the correlation between the HFI and the magnetic state of free standing Fe dimers, single Fe adatoms and dimers deposited on a bilayer of MgO(001). We find that the magnitude of the HFI can be controlled by switching the magnetic state of the dimers. For short Fe-Fe distances, the antiferromagnetic state enhances the HFI with respect to that of the ferromagnetic state. By increasing the distance between the magnetic atoms, a transition toward the opposite behavior is observed. Furthermore, we demonstrate the ability to substantially modify the HFI by atomic control of the location of the adatoms on the substrate. Our results establish the limits of applicability of the usual hyperfine hamiltonian and we propose an extension based on multiple scattering processes.

Noncollinear magnetism in two-dimensional CrTe2.

The discovery of two-dimensional (2D) van der Waals magnets opened unprecedented opportunities for the fundamental exploration of magnetism in quantum materials and the realization of next generation spintronic devices. Here, based on a multiscale modelling approach that combines first-principles calculations and a Heisenberg model supplied with ab-initio parameters, we report a strong magnetoelastic coupling in a free-standing monolayer of CrTe2. We demonstrate that different crystal structures of a single CrTe2give rise to non-collinear magnetism through magnetic frustration and emergence of the Dzyaloshinskii-Moriya interaction. Utilizing atomistic spin dynamics, we perform a detailed investigation of the complex magnetic properties pertaining to this 2D material impacted by the presence of various types of structural distortions akin to charge density waves.

Controlling in-gap end states by linking nonmagnetic atoms and artificially-constructed spin chains on superconductors.

Chains of magnetic atoms with either strong spin-orbit coupling or spiral magnetic order which are proximity-coupled to superconducting substrates can host topologically non-trivial Majorana bound states. The experimental signature of these states consists of spectral weight at the Fermi energy which is spatially localized near the ends of the chain. However, topologically trivial Yu-Shiba-Rusinov in-gap states localized near the ends of the chain can lead to similar spectra. Here, we explore a protocol to disentangle these contributions by artificially augmenting a candidate Majorana spin chain with orbitally-compatible nonmagnetic atoms. Combining scanning tunneling spectroscopy with ab-initio and tight-binding calculations, we realize a sharp spatial transition between the proximity-coupled spiral magnetic order and the non-magnetic superconducting wire termination, with persistent zero-energy spectral weight localized at either end of the magnetic spiral. Our findings open a new path towards the control of the spatial position of in-gap end states, trivial or Majorana, via different chain terminations, and the realization of designer Majorana chain networks for demonstrating topological quantum computation.

Comparative study of methodologies to compute the intrinsic Gilbert damping: interrelations, validity and physical consequences.

Relaxation effects are of primary importance in the description of magnetic excitations, leading to a myriad of methods addressing the phenomenological damping parameters. In this work, we consider several well-established forms of calculating the intrinsic Gilbert damping within a unified theoretical framework, mapping out their connections and the approximations required to derive each formula. This scheme enables a direct comparison of the different methods on the same footing and a consistent evaluation of their range of validity. Most methods lead to very similar results for the bulk ferromagnets Fe, Co and Ni, due to the low spin-orbit interaction (SOI) strength and the absence of the spin pumping mechanism. The effects of inhomogeneities, temperature and other sources of finite electronic lifetime are often accounted for by an empirical broadening of the electronic energy levels. We show that the contribution to the damping introduced by this broadening is additive, and so can be extracted by comparing the results of the calculations performed with and without SOI. Starting from simulated ferromagnetic resonance spectra based on the underlying electronic structure, we unambiguously demonstrate that the damping parameter obtained within the constant broadening approximation diverges for three-dimensional bulk magnets in the clean limit, while it remains finite for monolayers. Our work puts into perspective the several methods available to describe and compute the Gilbert damping, building a solid foundation for future investigations of magnetic relaxation effects in any kind of material.

Stabilizing spin systems via symmetrically tailored RKKY interactions.

Spins of single atoms adsorbed on substrates are promising building blocks for spintronics and quantum computation schemes. To process spin information and for increased magnetic stability, these spins have to be coupled to arrays. For a single atom, a high symmetry of the environment increases its spin stability. However, little is known about the role of the symmetry of the magnetic couplings in the arrays. Here, we study arrays of atomic spins coupled via Ruderman-Kittel-Kasuya-Yosida interaction, focusing on Dzyaloshinskii-Moriya and symmetric anisotropic exchange. We show that the high spin stability of a trimer can be remotely detected by a nearby atom, and how the Dzyaloshinskii-Moriya interaction leads to its destabilization. Adding more nearby atoms further destabilizes the trimer, due to a non-local effective transverse anisotropy originating in the symmetric anisotropic exchange. This transverse anisotropy can be quenched for highly symmetric structures, where the spin lifetime of the array increases drastically.

Complex magnetism of B20-MnGe: from spin-spirals, hedgehogs to monopoles.

B20 compounds are the playground for various non-trivial magnetic textures such as skyrmions, which are topologically protected states. Recent measurements on B20-MnGe indicate no clear consensus on its magnetic behavior, which is characterized by the presence of either spin-spirals or three-dimensional objects interpreted to be a cubic lattice of hedgehogs and anti-hedgehogs. Utilizing a massively parallel linear scaling all-electron density functional algorithm, we find from full first-principles simulations on cells containing thousands of atoms that upon increase of the compound volume, the state with lowest energy switches across different magnetic phases: ferromagnetic, spin-spiral, hedgehog and monopole.

Spin-fluctuation and spin-relaxation effects of single adatoms from first principles.

Single adatoms offer an exceptional playground for studying magnetism and its associated dynamics at the atomic scale. Here we review recent results on single adatoms deposited on metallic substrates, based on time-dependent density functional theory. First we analyze quantum zero-point spin-fluctuations (ZPSF) as calculated from the fluctuation-dissipation theorem, and show how they affect the magnetic stability by modifying the magnetic anisotropy energy. We also assess the impact of ZPSF in the limit of small hybridization to the substrate characteristic of semi-insulating substrates, connecting to recent experimental investigations where magnetic stability of a single adatom was achieved for the first time. Secondly, we inspect further the dynamics of single adatoms by considering the longitudinal and transverse spin-relaxation processes, whose time-scales are analyzed and related to the underlying electronic structure of both the adatom and the substrate. Thirdly, we analyze spin-fluctuation modes of paramagnetic adatoms, i.e. adatoms where the Stoner criterion for magnetism is almost fulfilled. Interestingly, such modes can develop well-defined peaks in the meV range, their main characteristics being determined by two fundamental electronic properties, namely the Stoner parameter and the density of states at the Fermi level. Furthermore, simulated inelastic scanning tunneling spectroscopy curves reveal that these spin-fluctuation modes can be triggered by tunneling electrons, opening up potential applications also for paramagnetic adatoms. Lastly, an overview of the outstanding issues and future directions is given.

Dynamical amplification of magnetoresistances and Hall currents up to the THz regime.

Spin-orbit-related effects offer a highly promising route for reading and writing information in magnetic units of future devices. These phenomena rely not only on the static magnetization orientation but also on its dynamics to achieve fast switchings that can reach the THz range. In this work, we consider Co/Pt and Fe/W bilayers to show that accounting for the phase difference between different processes is crucial to the correct description of the dynamical currents. By tuning each system towards its ferromagnetic resonance, we reveal that dynamical spin Hall angles can non-trivially change sign and be boosted by over 500%, reaching giant values. We demonstrate that charge and spin pumping mechanisms can greatly magnify or dwindle the currents flowing through the system, influencing all kinds of magnetoresistive and Hall effects, thus impacting also dc and second harmonic experimental measurements.

Chirality-driven orbital magnetic moments as a new probe for topological magnetic structures.

When electrons are driven through unconventional magnetic structures, such as skyrmions, they experience emergent electromagnetic fields that originate several Hall effects. Independently, ground-state emergent magnetic fields can also lead to orbital magnetism, even without the spin-orbit interaction. The close parallel between the geometric theories of the Hall effects and of the orbital magnetization raises the question: does a skyrmion display topological orbital magnetism? Here we first address the smallest systems with nonvanishing emergent magnetic field, trimers, characterizing the orbital magnetic properties from first-principles. Armed with this understanding, we study the orbital magnetism of skyrmions and demonstrate that the contribution driven by the emergent magnetic field is topological. This means that the topological contribution to the orbital moment does not change under continuous deformations of the magnetic structure. Furthermore, we use it to propose a new experimental protocol for the identification of topological magnetic structures, by soft X-ray spectroscopy.